Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

Wenchao Shangguan, Qing Liu, Ying Wang (), Ning Sun, Yu Liu, Rui Zhao, Yingxuan Li (), Chuanyi Wang and Jincai Zhao
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Wenchao Shangguan: Shaanxi University of Science and Technology
Qing Liu: Shaanxi University of Science and Technology
Ying Wang: State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences
Ning Sun: Shaanxi University of Science and Technology
Yu Liu: Zhengzhou University
Rui Zhao: Zhengzhou University
Yingxuan Li: Shaanxi University of Science and Technology
Chuanyi Wang: Shaanxi University of Science and Technology
Jincai Zhao: Key Laboratory of Photochemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Achieving CO2 reduction with H2O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO2 to CO with the help of H2O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g−1 h−1 (~100% selectivity), ~2.5 times the rate during CO2 reduction with H2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H2O decomposition, which synchronously optimizes the rate-determining steps in the CO2 reduction and H2O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO2 reduction with H2O.

Date: 2022
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DOI: 10.1038/s41467-022-31474-2

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